To elucidate the fundamental structure–property relationship of inhomogeneous polymer networks with different numbers of trapped entanglements, we have analyzed the mechanical properties and network structures of end-cross-linked star elastomers in the cross-linking procedure by coarse-grained molecular dynamics simulations and a graph-based structural analysis. From graph structural analysis based on the Scanlan–Case criterion, we identified the “effective chains” after excluding mechanically redundant network strands (loops, bridge centers, and dangling chains). The elastic moduli of the networks without trapped entanglements were not directly proportional to the number of effective chains but were proportional to the number of closed cycles formed by effective chains, in agreement with the phantom network theory. For networks with trapped entanglements, it was clarified that the elastic moduli can be predicted by a linear combination of the number of effective cycles and the number of entanglements formed by the effective chains, as expected by Langley’s formulation.

中文翻译：

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通过粗粒分子动力学模拟对具有大量捕获缠结的末端交联星形弹性体的线性弹性进行结构分析


为了阐明具有不同数量的捕获缠结的非均质聚合物网络的基本结构-性能关系，我们通过粗粒分子动力学模拟和分析了交联过程中末端交联的星形弹性体的力学性能和网络结构。基于图的结构分析。通过基于 Scanlan-Case 准则的图结构分析，我们在排除机械冗余的网络链（循环、桥中心和悬空链）后确定了“有效链”。没有陷阱纠缠的网络的弹性模量不与有效链的数量成正比，而是与有效链形成的闭环的数量成正比，这与幻影网络理论一致。对于具有捕获纠缠的网络，可以明确的是，弹性模量可以通过有效循环数和有效链形成的纠缠数的线性组合来预测，正如兰利公式所预期的那样。